Supplemental Packs (1961-1965)
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Before we begin, note that I'm not going through every single pack individually, as we can be a lot more efficient and cover everything at once.
Introduction
Along with the wider wave of sets that debuted in North America in 1961, there were also a healthy range of supplements available. The below table is from the earliest pamphlet, showing each part and all available colors, as well as some errors and omissions which we will go over:

The pamphlet isn't exactly indicative of availability, as for example, the 235 Garage never came with a white door in North America, it used a red door. The trees experienced something similar, as later examples used Samsonite's own unpainted versions but the image was not updated. Then there are things that I'm not sure about, such as the swing for the 214's doors, whether or not they were right or left or ever consistent.
But before we go too far down the rabbit hole, let's go over the boxes and their variants, as that's by far the most interesting part for me. For the completionists, if you want to have every possible variant, this is by far the biggest hurtle to overcome.
Boxes/Variants
There are two major differences between boxes depending on if they were produced earlier or later. 1961-62 examples will say "Pat Pend" and lack registered trademark symbols. 1963-65 examples will list two patents & have registered trademark symbols:
Also worthy of note, the image on the front was randomized, shown in this article are four different possible images:
I'm not sure whether or not there were more possible images not shown here.
Regardless, in considering a complete collection with all variants, there were well over one hundred different supplemental boxes without accounting for any box variations, and with the above information, there are as many as 800. But that's not the worst of it.
Each box also had their country of origin printed on it, meaning Canadian supplements had "Printed in Canada" instead of "Printed in USA" on them, meaning there are potentially 1200+ different box variants. It'd be next to impossible to collect them all, at least not without significant investment.
With that covered, each box had a generic side:

And the tabs would give the set number, a trailing letter (to differentiate part variations within a family, i.e. 1x6/8 bricks, windows, etc.)

Only one of the supplements came with instructions: the 245 Lighting Device:
1963 Expansion
In 1963, in both the US and Canada, the supplements line expanded immensely. With the 1963 release of the 605 Wheel Toy and the 905 Doll Set, black LEGO elements were introduced into North America. The same is true for flat plates smaller than 2x8 (1x1, 1x2, 2x2, 2x4).
As a result, all basic brick supplements had a black version introduced, as well as the smaller flat plates in a wide variety of colors.
Also introduced in 1963, both to North America and the supplements line, was the 400 Wheel Supplement. It sold at a slightly higher 75c price and came with a few plates as well as a tow plate:

A fairly decent representation of the full 1963 line can be found in 1963 brochures:

Though there is one specific thing I want to call out: the 4x4 corner brick.
Take a look at the 4x4 corner bricks listing above, notice that it has two colors exclusive to North America: black and trans-clear.
Wait, trans-clear?!
Yes, for some bizarre reason, the above supplements lists trans-clear as having been an available color for the 4x4 corner bricks. And I say bizarre because I'm not aware of any surviving examples of that specific color, let alone any boxes. I'm extremely confident they were never produced in that color, at least not for mass retail. If just one example of a trans-clear 4x4 corner brick appeared, I'd moreso believe it to have been a non-production element rather than from a supplement pack that sold in a store.
But it is interesting that Samsonite never corrected that if it truly was not available, as the supplement list was updated in both 1964 and 1965. It could very well be one of those discrepencies between Samsonite employees who planned, employees who prepared materials, and those who actually worked production lines.
Remember, for this time USA Samsonite was at the mercy of their Canadian subsidiary for part production, meaning that they could only sell whatever the parts that were shipped to them. And Samsonite of Canada never advertised the 4x4 corner brick coming in clear, so it is highly unlikely clear was an actual available color in the USA.
That mystery is one the earliest things I'd ever properly looked into in the LEGO Samsonite realm, back when I first started collecting. Before and since then, I've oddly never seen it discussed. But beyond what we've covered above, there's not really more to discuss or mull over, beyond saying "no one has seen one" and shrugging our shoulders.
1964 Expansion
Technically, the Individual 1:87 Cars were also part of this supplemental line. They are seen in 1964-65 materials:

If you wish to learn more about those in particular, follow the article linked above. To summarize, there were six different vehicles available in North America and sold for 75c in a clear garage:

Canadian Exclusives
To my knowledge, Samsonite of Canada had the same supplemental line as the US. They both shared the same LEGO factory during 1961-64, so there's not much reason to assume dissonance. Though it's always possible, as seen below.
Exclusive to the Canadian market was the larger wheel supplement, the 401 Large Wheel Supplement:

Presumably, it released in Canada concurrently with the 610 Super Wheel Toy in 1964, but the earliest I've found it appearing in media is 1965.
Canada also exclusively sold the 402 Swivels and Base Plates supplement.
I'm not sure why the US market skipped the 401 and 402. Perhaps it had to do with the Detroit plant closing in 1964 (where LEGO packaging was produced before Loveland opened in early 1965), or maybe it stemmed from the supplement line's overall performance. Speaking of which:
Troublesome Sales
The 1961-65 supplements, at least in the USA, often struggled to sell at full retail. It's not necessarily to do with complete buyer disinterest, but instead a struggle for retailers to sell odd parts packs. Remember there were over a hundred different possible parts/colors, many of which were exclusive to the supplements line and not part of assortments within sets.
It was such an issue that Samsonite felt the need to address the massive change when the supplements line was reconfigured in 1966: "LEGO announces a completely new extra parts program.... The number of boxes in the extra parts line has been reduced from 144 to 14, including only the most popular assortments."
To flush the remaining stock of the supplements parts, Samsonite created the 695 Bulk Assortment Set. Notice how between examples, even though supplements had tons of different pieces and colors, several pieces reappear across examples such as white macaroni bricks:

