To contradict the theory of gravity before it was proven to be a law, the most compelling evidence would be:
Observations of objects floating upwards without any external force.
This would directly challenge the fundamental premise of gravity, which states that mass attracts mass and objects are pulled towards the center of Earth (or any mass). If objects were consistently observed to float upwards without an external force acting on them, it would imply that the gravitational force is not acting as predicted.