Optical and scintillation properties of CsCl:Tl and CsCl:In single crystals were investigated. Ions Tl+ and In+ were selected as dopants to enhance the light yield of CsCl crystals. Luminescence and scintillation spectra of CsCl:Tl and CsCl:In could be attributed to the relaxed excited state (RES) originating from each dopant ion. The decay-time constants of the fast component had values of 5.4 ns for CsCl:Tl and 2.2 ns for CsCl:In, and can be ascribed to the overlapping of on-center STE and auger-free luminescence (AFL) for CsCl:Tl and only AFL for CsCl:In, respectively. Decay-time constants of the slow component were relatively long (220 ns for CsCl:Tl and 240 ns for CsCl:In), possibly owing to their low energy transfer rate from host to each dopant ion. The light yields of CsCl:1%Tl and CsCl:0.5%Tl were estimated to be 2800 and 2200 photons/MeV, respectively. The light yield of CsCl:0.5%In crystals was estimated to be 2200 photons/MeV. In conclusion, the light yield of pure CsCl (several ten photons/MeV) can be enhanced by doping Tl+ and In+ while maintaining the fast component of the CsCl crystal.