The influence of adding surfactants on the performance of high-solid anaerobic digestion of horticultural waste was extensively investigated in batch systems. Adding Tween series and polyethylene glycol series non-ionic surfactants had positive effects on biogas production, resulting in 370.1 mL/g VS and 256.6 mL/g VS with Tween 60 and polyethylene glycol 300 at a surfactant-to-grass mass ratio of 0.20, while the biogas production of anaerobic digestion without surfactants was 107.54 mL/g VS. The optimal and economically feasible choice was adding Tween 20 at a ratio of 0.08 g/g grass in high-solid anaerobic digestion. A kinetics model reliably represented the relationship between surfactant concentration and biogas production. The mechanism of surfactants working on lignocellulose was investigated. The improvement in high-solid anaerobic digestion by adding surfactants was attributed to the interaction between lignocelluloses and surfactants and the extraction of biodegradable fractions from the porous structure. An economic analysis showed that adding Tween 20 was likely to make a profit and be more feasible than adding Tween 60 and polyethylene glycol 300. This study confirms the enhancement in biogas production from horticultural waste by adding non-ionic surfactants.