Straw return and plastic film mulching are two critical management measures that not only maintain high and stable crop yields, but also have a significant impact on the ecological environment. However, there is still a lack of research on the comprehensive effects of straw return and different film mulching treatments on the ecological environment. Thus, a 2-year field experiment was conducted and six treatments, which included two main treatments, namely straw return (SR) and non-straw return (NR), and three sub-treatments, namely no film mulching (CK), plastic film mulching (PM) and fully biodegradable film mulching (BM), were applied in a garlic cropping system. Based on the life cycle assessment method, six endpoint damage categories, resource consumption, global warming potential, environmental acidification, eutrophication, human health, and ecotoxicity, were assessed. Furthermore, we also evaluated the costs and economic benefits of the six treatments and optimized the treatment of used mulch and straw off-farm. The results indicated that the environmental impacts of the six endpoint damages in the garlic cropping system were ranked as ecotoxicity, eutrophication, environmental acidification, global warming potential, human health, and resource consumption. The SR-BM treatment had the lowest life cycle environmental impact composite index at 27.68 per unit area, followed by SR-PM at 27.75. All six endpoint damage categories for the PM and BM treatments were lower than the CK treatment per t of yield, with the SR-BM treatment being the most economically efficient, yielding at 3691.03 CNY·t−1 and exceeding that of the SR-CK treatment by 7.26%. Fertilizer inputs were the primary contributor to resource consumption, global warming potential, environmental acidification, eutrophication, and ecotoxicity, accounting for about 72.80% of these five environmental impacts. Crop protection significantly affected human health, and garlic mulching helped minimize pesticide use, thereby reducing potential health impacts. Compared to straw incineration and waste mulch power generation, straw power generation and waste mulch recycling granulation offered positive environmental benefits and were more effective offset strategies. In conclusion, straw return with biodegradable mulch is a synergistic cultivation measure that offers both environmental and economic benefits. For straw return with plastic film mulch, environmental impacts can be reduced by waste mulch recycling granulation.
