Diagnostics with three-dimensional (3D) spatial resolution and rapid temporal resolution have been long desired to resolve the complicated turbulence-chemistry interactions. This paper describes a method based on based on tomographic chemiluminescence (TC) to address this diagnostic need. The TC technique used multiple cameras to simultaneously record CH* chemiluminescence emitted by turbulent flames from different view angles. A 3D tomographic algorithm was then applied to reconstruct the instantaneous flame structures volumetrically. Both experimental and computational studies have been conducted to demonstrate and validate the 3D measurements. Experimental results were obtained instantaneously at kHz temporal rate, in a volume of 16 × 16 × 16 cm3, and with a spatial resolution estimated to be 2~3 mm. Computations were conducted to simulate the experimental conditions for comparison and validation.