Those temps are not that high. Chill only caps the framerate and drops it when you don't move much in a game or the game has less movement scenes.
What case do you have? Can you monitor the temperatures with CPUID HWMonitor so we can see better the rest of the system temperatures?
Describe the rest of your hardware and what version of Windows and drivers are you using.
You can try to adjust Chill to your monitor framerate and see how it goes.
EDIT: Check this video Radeon™ Software: How-To Use Radeon™ Chill - YouTube