Recent advances in power scaling of fiber lasers are hindered by the thermal issues, which deteriorate the beam quality. Anti-Stokes fluorescence cooling has been suggested as a viable method to balance the heat generated by the quantum defect and background absorption. Such radiation-balanced configurations rely on the availability of cooling-grade rare-earth-doped gain materials. Herein, we perform a series of tests on an ytterbium-doped ZrF4–BaF2–LaF3–AlF3–NaF (ZBLAN) optical fiber to extract its laser-cooling-related parameters and show that it is a viable laser-cooling medium for radiation balancing. In particular, a detailed laser-induced modulation spectrum test is performed to highlight the transition of this fiber to the cooling regime as a function of the pump laser wavelength. Numerical simulations support the feasibility of a radiation-balanced laser, but they highlight that practical radiation-balanced designs are more demanding on the fiber material properties, especially on the background absorption, than solid-state laser-cooling experiments.