ZnOS phosphors were synthesized by a two-step high-temperature solid-phase method. The as-synthesized CaS:Eu 2+ ,Pb 2+ @Ca-ZnOS:Pb 2+ phosphors possess excellent dual-excitation and dualemission (DE 2 ) luminescent properties, which give rise to red emission peaking at 650 nm under green excitation, derived from the core CaS:Eu 2+ ,Pb 2+ , and blue emission peaking at 424 nm, originating from the shell CaZnOS:Pb 2+ , under ultraviolet (UV) excitation. In addition, tunable red/blue emission can be achieved by changing the doping concentration of Pb 2+ in the CaZnOS shell. The red/blue dual emission of core−shell DE 2 phosphors under excitation of UV and green light significantly matches with the absorption spectrum of chlorophyll (a, b); hence, the as-prepared phosphors are excellent solar spectral conversion (SSC) auxiliaries of plastic films or laminated glass for greenhouses and provide ideas for creating more efficient and practically valuable SSC auxiliaries. The DE 2 properties are described, and the energy transfer mechanism from Pb 2+ to Eu 2+ in the core is proposed and discussed in detail.