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Organic substances of low biodegradability and the high moisture content of herbaceous peat inhibit its high-value utilization. In this study, the effect of pretreatment with dilute sulfuric acid on the efficiency of the anaerobic fermentation of herbaceous peat was explored. Single-factor experiments and orthogonal tests were conducted to optimize the pretreatment conditions. The milled herbaceous peat (0.43 mm) was pretreated with 5% sulfuric acid at 100°C for 120 min with a solid–liquid ratio of 1:4, and the reducing sugar yield was 13.49%. The results suggest that dilute sulfuric acid might have hydrolyzed the β-glycosidic bonds between the sugar monomers, causing the partial degradation of cellulose into reducing sugar. Compared to the fermentation of untreated herbaceous peat, the total biomethane yield increased by 29.97%, and the fermentation period decreased by 22.50%. Thus, pretreatment with dilute sulfuric acid effectively enhanced the efficiency of biomethane fermentation of herbaceous peat.