The most compelling evidence that would have contradicted the theory of gravity before it was proven to be a law would be observations of objects floating upwards without any external force. This would directly challenge the principle of gravity, which asserts that masses are attracted towards each other. If objects consistently floated upwards without an external force, it would indicate that gravitational attraction was either not acting as proposed or was being counteracted by an unknown mechanism.
Other options, such as discovering a stronger universal force or variations in the gravitational constant, could suggest modifications to our understanding of gravity but would not outright negate the existence of gravity itself. Similarly, experiments showing different masses falling at different rates in a vacuum would contradict a specific aspect of gravitational theory but wouldn't fully refute gravity as a whole.