We report the complete characterization of various cooling-grade Tm-doped crystals including, to the best of our knowledge, the first demonstration of optical refrigeration in Tm:YLF crystals. Room temperature laser cooling efficiencies of 1% and 2% (mol) Tm:YLF and 1% Tm:BYF crystals at different excitation polarizations are measured, and their external quantum efficiency and background absorption are extracted. By performing detailed low-temperature spectroscopic analysis of the samples, global minimum achievable temperatures of 160 to 110 K are estimated. The potential of Tm-doped crystals to realize mid-IR optical cryocoolers and radiation balanced lasers (RBLs) in the eye-safe region of the spectrum is discussed, and a promising two-tone RBL in a tandem structure of Tm:YLF and Ho:YLF crystals is proposed.