Thallium bromide (TlBr) and thallium chloride (TlCl) are semiconductor materials with high transparency to visible light, high index of refraction, and high detection efficiency for gamma rays and annihilation photons. This manuscript reports on measurements of the light intensity and timing response of Čerenkov light emitted in one 3 mm × 3 mm × 5 mm slab of each of these materials operated in coincidence with a lutetium fine silicate (LFS) crystal with dimensions of 3 mm × 3 mm × 20 mm. A 22Na radioactive source was used. The measured average number of detected photons per event was 1.5 photons for TlBr and 2.8 photons for TlCl when these materials were coupled to a silicon photomultiplier. Simulation predicts these results with an overestimation of 12%. The best coincidence time resolution (CTR) for events in TlBr and TlCl were 329 ± 9 ps and 316 ± 9 ps, respectively, when events with 4 photons and >7 photons were selected. Simulation showed the CTR degraded from 120 ps to 405 ps in TlCl, and from 160 ps to 700 ps in TlBr when the first or second Čerenkov photon were selected. Results of this work show TlCl has a stronger Čerenkov light emission compared to TlBr and a greater potential to obtain the best timing measurements. Results also stress the importance of improving detection efficiency and transport of light to capture the first Čerenkov photon in timing measurements.