So just to clarify you have an animation of a 3d ball rolling and you want it to be syncronized with the motion of the ball?
In the simple case of having an animation of the ball rolling to the right you can set the angle to be the same as the angle of motion as you have above.
The second thing to do is correlate the animation speed with the speed of the object's motion.
So depending on the number of frames you can find the time for a full rotation with:
So we can the find angular speed with:
Which then solves to:
You can then relate linear speed to rotations with:
Then combining the two:
And solving for animation speed we get our formula:
Speed can be calculated as you have.
Radius is half the width of the ball.