The role of total solids content in low-temperature thermal hydrolysis and anaerobic digestion of sewage sludge was investigated. Increasing total solids from 2% to 6% improved thermal hydrolysis and anaerobic digestion performance, while increasing it further to 12% decreased methane production. Maximum sludge solubility (22.9% ± 0.6%) and methane production (320 ± 7 mL/g volatile solids) were achieved at 6% solids. The increase in solids content from 2% to 6% improved heating efficiency and volatile fraction content, which facilitated sludge solubilization and enrichment of methanogens. However, further increases in solids content resulted in a stable floc structure with excess ammonia nitrogen and volatile fatty acids, which limited the release of substrates and reduced the abundance of acidifying bacteria and methanogens, ultimately leading to reduced methane production. An in-depth understanding of the role of solids content opens up new avenues for improved low-temperature thermal hydrolysis of sludge.