Avoid unless you’re a tech hobbyist curious about extreme compression methods (like dummy file removal or ROM hacking). For actual PS2 gaming, stick to standard ISOs (1–3GB) or original hardware. 100MB might give you a playable Atari 2600 game, not Shadow of the Colossus.
After scouring compression forums (7z, ZIP, CSO Level 9), here are legitimate titles that fit the bill. These are not demos; they are full retail games that were just very small to begin with.
To play these files, you will need a PS2 emulator. The hardware requirements for PS2 emulation are higher than older consoles like the GameCube or PSP, but modern mid-range devices can handle it well.