In this study, a type of artificial lightweight shale ceramsite (ALSC) was used as the coarse lightweight aggregate for shotcrete (LAS), of which the mechanical properties, chloride penetration ion resistance, and rebound behavior were investigated. Based on the experimental results on compressive, tensile, and bond strength, LAS meet the strength requirements, and the replacement rate of fly ash (FA) and silica fume (SF) are suggested to be kept at ~15% and 10%, respectively, to result in the best mechanical properties of LAS. Adding FA and SF to the mixture significantly improved the chloride ion penetration resistance (CPR) of LAS because of morphology effects and secondary hydration of FA and SF that lead to a denser microstructure of the mixture. The electric flux and chloride ion migration coefficient (DRCM) of LAS decreased by 56% and 67%, respectively, with FA increasing from 0 to 10%. The electric flux and DRCM further decreased by 71% (153C) and 66% (3.24 m2/s), respectively, with FA increasing from 10 to 20%. As 5–10% SF was further added, the electric flux and DRCM of LAS decreased to extremely low levels; for instance, with FA = 10% and SF = 10%, DRCM = 1.61 m2/s, and the electric flux was too small and could be ignored. The contact stresses between aggregate and shotcrete mixtures were measured to investigate the rebound trend of ALSC in shotcrete. According to the analyses of the theoretical model of the rebound behavior of aggregate in shotcrete proposed by Armelin and Banthia, because of the reduced contact stresses between ALSC and mortar and the smaller density of LAS compared with normal-weight aggregate, the rebound rate of ALSC was about half of that of normal-weight aggregate in the shooting process of the shotcrete.