Poplar wood was treated with peracetic acid, KOH, and ball milling to produce 147 modellignocelluloses with a broad spectrum of lignin contents, acetyl contents, and crystallinity indices (CrIs), respectively. An empirical model was identified that describes the roles of these three properties in enzymatic hydrolysis. Lignin content and CrI have the greatest impact on biomass digestibility, whereas acetyl content has a minor impact. The digestibility of several lime-treated biomass samples agreed with the empirical model. Lime treatment removesallacetyl groups and a moderate amount of lignin and increases CrIslightly; lignin removal is the dominant benefit from lime treatment.