head to head
Neither is simply harder - they are hard in different places. Left 4 Dead demands more reads; The Binding of Isaac demands more variance.

Execution · Twitch Chaos
Co-op zombie shooter whose AI Director reshuffles every run to keep teams honest.

Execution · Twitch Chaos
Twin-stick roguelike where a crying child fights basement horrors with random unholy upgrades.
Left 4 Dead leans Execution (Twitch Chaos); The Binding of Isaac leans Execution (Twitch Chaos).
Same score on execution - which means the number cannot separate them. The difference is in what each one asks of you.
Left 4 Dead
Headshots, melee shoves, and special-infected reaction time
The Binding of Isaac
Twin-stick dodging through bullet-dense rooms
Left 4 Dead leans clearly harder on reads.
Left 4 Dead
Versus mode adds human ambush mindgames
The Binding of Isaac
Enemies follow fixed or random patterns
The Binding of Isaac leans clearly harder on variance.
Left 4 Dead
AI Director randomizes hordes, items, and specials
The Binding of Isaac
Item and room RNG defines every run
The Binding of Isaac leans a little harder on optimization, though the gap is small.
Left 4 Dead
Team spacing, route choice, and resource discipline
The Binding of Isaac
Item synergy knowledge converts luck into wins
A matching score does not mean a matching test. Two games can both sit at 10 on execution and demand completely different things of you - which is why the reasoning above matters more than the number beside it.