First, if your NEC 220.82 Load Calculation is currently 90 amps on a 100A service, you will not be adding 60A of additional load... except using a load management technique. This is easier or harder, depending on whether the load is a dumb load like a hot tub, or a smart load like an EV. (guess what we get a lot of requests for... speaking of EVs, 50/60A is crazy overkill if you're not a hotel, see Technology Connections' primer on the subject particularly 28:15 and 32:55.)
Now you're saying your main "panel" only has one breaker. It sounds like a "Meter-Main. It's possible to tee off that, but it's annoying, and will involve at least $100 worth of Polaris connectors. It's fine to treat your "main subpanel" as if it's a main panel for this discussion. For the Load Management stuff, it doesn't matter that much whether you go to the meter-main or the "one with all your breakers", however it's going to get pretty crowded in that meter-main with both 3 Polaris splices and also the load management box.
I recommend that conduit be built legally (built empty and the wires pulled in) despite the added expense. Because #1 you're going to need that load management system, and it'll need data wires. And #2 if it's EV, Vehicle 2 Home is right around the corner, and we have no earthly idea which wires will be required for that (HVDC cables?) I would recommend 1" conduit, or preferably, 1-1/4" conduit.
Once that's in, decide which wire suits your budget - for 60A either #6 copper or #2 aluminum individual wires in the conduit. If you go with cable, just go 2-2-2-4 aluminum, though #6 copper SER (not NM) would suffice.
If this is for basic at-home EV charging, you could side-step the Load Management equipment by simply turning charge rate down to sensible levels for home charging. Adopt an ABC "Always Be Charging" strategy (within favorable energy tariffs if possible). That simply requires 12/2 cable from a 15A/240V breaker to a suitable location in the garage for a "wall unit" (the classy kind you see in the commercials). Configure the wall unit for 15A breaker/12A actual charge, and done. This is more than twice the speed of level 1, plenty for most people.