Novel Ho3+ doped highly transparent NaYbF4 glass-ceramics were successfully fabricated by melt-quenching technique. Their structural and luminescent properties were systemically investigated by XRD, TEM, absorption spectra, upconversion spectra, and lifetime measurements. Excited by 980-nm laser, samples exhibit characteristic emissions of Ho3+. Impressively, the luminescent color can be tuned easily from red for precursor glass to green for glass-ceramics. Such novel phenomenon was elaborately investigated and is owing to the reduced multiphonon nonradiative relaxation and enhanced cross-relaxation of Ho3+ in NaYbF4 nanocrystals after crystallization. Our results indicate that NaYbF4 transparent glass-ceramics is an excellent host for upconversion.