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The coal gangue coarse-aggregate content in ordinary concrete should not be too large. In order to further improve the utilization rate of coal gangue coarse aggregate, this study used the principle of "strong wrapped weak" to prepare high-performance concrete. This study considered four factors, namely, water–binder (W/B) ratios, non-spontaneous combustion coal gangue (NCCG) coarse-aggregate contents, fly ash–slag mass ratios, and silica fume coating to prepare high-performance concrete. The workability, mechanical, and durability properties were studied, and the changes in the interfacial transition zone (ITZ) of concrete before and after sulfate attack and freeze–thaw cycles were analyzed based on the SEM test. The life prediction of NCCG coarse-aggregate high-performance concrete was carried out based on the grey system GM(1,1) prediction model. The results show that the NCCG coarse-aggregate contents have the greatest effect on compressive strength, sulfate resistance, and frost resistance. The W/B ratio has the greatest effect on the anti-carbonization properties. Fly ash–slag mixing can obtain better durability. Considering the effect on the design service life of high-performance concrete, NCCG coarse aggregate is used to prepare high-performance concrete in North China, and the recommended content is 60%; in the Northwest and Northeast regions, the recommended content is 45%. This study provides a basis for the preparation of high-performance concrete with NCCG coarse aggregate. [ABSTRACT FROM AUTHOR]