Broadband sensitization is an effective strategy to enhance the upconversion luminescence (UCL) of lanthanide ions.Herein,novel UC materials LiScSi2O6∶Cr3+/Er3+ (LSS∶Cr3+/Er3+) were synthesized by high-temperature solid state reaction and their luminescent properties were investigated.LSS∶Cr3+/Er3+has the broadband absorption in the spectral range of 600-800 nm,and meanwhile shows green UC emissions of Er3+ upon pumping Cr3+ by the 690 nm laser.The UCL of LSS∶Cr3+/Er3+ belongs to the two-photon process and is attributed to the energy transfer upconversion mechanism.The effects of the Cr3+and Er3+ concentration as well as the Yb3+ introduction were also studied.LSS∶Cr3+/Yb3+/Er3+ exhibits the interesting dual-mode UCL,capable of generating the UCL of Cr3+ upon pumping Yb3+ ions and the UCL of Er3+ upon pumping Cr3+ ions.This research might promote the development of novel broadband Cr3+-sensitized UC materials.