Gasification slag (GS) is rich in SiO2, Al2O3, and Fe2O3, and has excellent particle size gradation, which has the potential to be employed as an aggregate in the field of controlled low-strength material (CLSM). Nevertheless, the large-scale application of GS as the fine aggregate for the preparation of CLSM has been scarcely investigated. In the present work, the applicability of replacing part of coal gangue (CG) with gasification coarse slag (GCS) as fine aggregate for the preparation of CLSM was investigated. The results revealed that using GCS as a fine aggregate improved the flowability of CLSM, and increasing the GCS content from 0 to 50 wt% improved the flowability from 250.0 to 280.0 mm. The 28-day compressive strength of all CLSM conformed to the requirements of ACI Committee 229. Compared to the Blank group, the 7- and 28-day compressive strength of the CLSM increased by 23.07% and 26.80%, respectively, at a GCS content of 50 wt%. The increase in compressive strength was mainly due to the pore-filling and hydration-promoting effect of the GCS, which made the structure denser. The dense structure reduced the expansion rate, absorption, and porosity rate of CLSM and increased the wet density. The optimal process parameter was the addition of 10 wt% of GCS. The results of heavy metal ion leaching showed that the optimal sample GS10 leached all heavy metal ions in much less than the limit values of GB 8978-1996 and GB 5085.3-2007. The results will provide new ideas and technical approaches for the large-scale application of GCS as the fine aggregate in CLSM.