This study explores the production of bio-nutrients from bioactive compound-rich spent coffee grounds (SCG) and biochar (BC) through composting after inoculation with a biological agent and its impact on the growth performance of garden cress and spinach. The SCG was composted with six doses of BC (0, 5, 10, 15, 20, and 25%). The compost with 10% BC exhibited the best maturity, humification, and phytotoxicity index values of dissolved organic carbon (DOC), humification index (E4/E6), and germination index (GI). A metagenome analysis showed that compost starter enhanced the bacterial community’s relative abundance, richness, and diversity in SCG and BC treatments. This improvement included increased Patescibacteria, which can break down noxious phenolic compounds found in SCG and BC. The BC enriched the compost with phosphorus and potassium while preserving the nitrogen. In plant growth experiments, the total chlorophyll content in compost-treated garden cress and spinach was 2.47 and 4.88 mg g−1, respectively, which was significantly greater (p ≤ 0.05) than in unfertilized plants and similar to the plants treated with traditional fertilizer. Overall, the results show that the compost of SCG + BC was well-suited for promoting the growth of garden cress and spinach, providing adequate nutrients as a fertilizer for these leafy vegetables.