An ideal scintillator for X- and gamma-ray detection should have a high light yield and a high effective atomic number (Zeff). In this study, we developed undoped TlCdCl3 crystals and TlCdCl3:Sb (Sb: 0.5, 1.0 and 1.5 mol%) crystals with high Zeff (TlCdCl3:68.7), as candidate scintillators. The crystals were grown using the self-seeding solidification method, and their photoluminescence (PL) and scintillation properties were investigated. For the undoped TlCdCl3 crystals, emission peaks were observed at 460 nm and 485 nm in the PL and X-ray-induced radioluminescence (XRL) spectra, respectively. For the TlCdCl3:Sb crystals, the PL spectra showed emission peaks at 480, 480 and 500 nm, while the XRL spectra exhibited peaks at approximately 510 nm. The emission bands of the TlCdCl3:Sb crystals were shifted to longer wavelengths than those of the undoped TlCdCl3 crystals. The scintillation decay time constants for the undoped TlCdCl3 crystals were 51 and 2613 ns, whereas for the TlCdCl3:Sb crystals, they were in the range of 65–81 and 4550–7350 ns. These results suggest that the incorporation of Sb3+ ions induces long components of several thousand nanoseconds. The redshift and appearance of these long components indicate that Sb3+ ions act as new luminescence centers in the undoped TlCdCl3 crystal. The scintillation light yield of the TlCdCl3:Sb 1.0 mol% crystal was measured at 10,300 photons/MeV. The doping of Sb3+ ions into the TlCdCl3 lattice improved the scintillation light yield by up to four times compared to the undoped TlCdCl3 crystal.