An effective pathway to achieve the sustainable development of resources and environmental protection is to utilize shale ceramsite (SC), which is processed from shale spoil to produce high-strength lightweight concrete (HSLWC). Furthermore, the urgent demand for better performance of HSLWC has stimulated active research on graphene oxide (GO) in strengthening mechanical properties and durability. This study was an effort to investigate the effect of different contents of GO on HSLWC manufactured from SC. For this purpose, six mixtures containing GO in the range of 0–0.08% (by weight of cement) were systematically designed to test the mechanical properties (compressive strength, flexural strength, and splitting tensile strength), durability (chloride penetration resistance, freezing–thawing resistance, and sulfate attack resistance), and microstructure. The experimental results showed that the optimum amount of 0.05% GO can maximize the compressive strength, flexural strength, and splitting tensile strength by 20.1%, 34.3%, and 24.2%, respectively, and exhibited excellent chloride penetration resistance, freezing–thawing resistance, and sulfate attack resistance. Note that when the addition of GO was relatively high, the performance improvement in HSLWC as attenuated instead. Therefore, based on the comprehensive analysis of microstructure, the optimal addition level of GO to achieve the best mechanical properties and durability of HSLWC is considered to be 0.05%. These findings can provide a new method for the use of SC in engineering.