Upconversion materials with tunable emission colors are highly desired for novel anticounterfeiting strategies because they offer additional security features. Herein, we report a series of upconversion hybrids consisting of NaYF₄:Yb/Ln microrods (MRs) and NaGdF₄:Yb/Ln@NaYbF₄ (Ln = Er, Ce/Ho, Tm) core/active-shell nanocrystals (NCs). A normal thermal quenching of upconversion luminescence (UCL) is found for the MRs, but a thermal UCL enhancement occurs for the small-sized NCs. Consequently, the hybrids exhibit temperature-responsive multicolor emissions with large color shifts. The UCL enhancement mechanism is further revealed by temperature-dependent steady/transient spectral analysis in various atmospheres. Moreover, various color-shifting pathways are realized by adjusting the MR/NC combinations in the hybrids. Thanks to the effective photothermal conversion of core/active-shell NCs, color changes of the printed patterns by the hybrid ink are achieved simply by single-laser irradiation at a relatively low power density. These desirable properties make the designed hybrids promising for anticounterfeiting applications with advantages of high-level security and convenient authentication methods.