The playstyle looks human. Besides, it's always the same pattern, as he said himself. Some players can get a groove going and do something like this for an hour. I'm not saying your theory of it being a TAS is wrong. I'm just presenting the idea that it's possible that it's not tool-assisted; playing the devil's advocate. It does seem insane / extremely unlikely to me that any human could pull off the gameplay in the sixth part of that run, especially without a single death.
Stella, considered the best Atari 2600 emulator from a quick Google search, has a fully-featured
debugger for Atari 2600 games. I just got Stella to try it out, but I don't understand how to run the game in the debugger so it didn't go very well. This may be the key to whatever this guy may have done to make those videos.
Also, vmware workstation and vmware player have playback-syncing recording capabilities. They are also possible keys to the magic door of TASing Atari 2600 games.