A few thoughts:
Yes, it's frustrating to have to remember to stop by the hardware store for a bolt that you maybe should already have, but from someone who has a fairly large assortment of nuts, bolts, sheet metal screws, wood screws, lag bolts, "standard" nails, pneumatic nails, staples, etc., 90% or more of which are sorted, take your time, and figure out what is practical for YOU, because you'll most likely never reach the point that you still don't have something that you really need; at least I never have. I have to assume that you are a D.I.Y. guy, so you will spend more than enough on simple hardware over your lifetime, so don't waste it. And, just trying to think of an example of what I mean by "practical for you", I happen to like old tractors, and for whatever reason, 7/16 bolts and nuts are fairly common on them, so while I have many of them, you may never run into a need for a single one.
Consider the space that you have now, how you will sort them, and, since it sounds like you want to make some manner of "bulk purchase" to get yourself started, how you will store them. Some of the assortments come with neat bin boxes, that can be very useful, but are they what you have in mind? If not, an assortment that comes in bags may be better, and you can save your money to buy some lumber to build custom boxes.
PLAN FOR EXPANSION.
If you want to keep it more compact, the big boxes sell stackable divided units that set in a plastic 5 gallon bucket. I don't find them handy for use in my shop, but I have them, nevertheless, stocked with nails screws, etc. that I can quickly set in the truck to take on the road.
TSC and other places still sell bolts, nuts, etc. by the pound. Quality wise, I wouldn't use them to bolt in a clutch or exhaust manifold, but they are great for many things.
While you at it, and if applicable to the things that you do, don't forget to allow space for miscellaneous items such as snap rings, cotter pins, springs, spacers, wood dowels, biscuits, etc. As an example, I have a couple of places, depending on size, where I even keep scrap pieces of leather, copper, nylon, and other things that I might use at some point. It's easy to get carried away, but if you maintain a perspective on what the odds are of needing a particular item, you can have a great D.I.Y. inventory, without having the wife wanting to kick you out the door!