Traditionally, operational envelopes for anaerobic digestion (AD) have relied on empirical methods based on feedstock type. However, innovations like pre-treatment technologies challenge this norm by inducing partial degradation through hydrolysis, which breaks down macromolecules into bioavailable forms. In partnership with Anglian Water, this study develops a framework for optimizing AD with thermal hydrolysis pre-treatment (THP-AD) by assessing the impact of these technologies on feedstock composition and addressing optimization gaps with targeted enzyme dosing. THP pre-treatment enhances carbohydrate degradation and protein solubilization, though some proteins remain solubilized without converting to biogas. Enzymes targeting protein hydrolysis boost biogas yield by 16-33% in THP-AD batch reactors. In continuous THP-ADs, low-cost protein-targeting enzymes reduced total proteins by 10% and increased soluble organics by 15-25%, ammonia by 15-20%, and long-chain fatty acids by 10-20%. The findings indicate a potential 30% increase in biogas production using hydrolysis enzymes to tackle the hydrolysis gap created by THP pre-treatment. This further conversion of soluble carbon to methane could help meet the Industrial Emissions Directive (IED) requirements, addressing concerns about increased volatile fatty acids and soluble chemical oxygen demands, which are roughly 7 to 15 times greater than conventional AD per unit of volatile solids in the digestate.