Hydrothermal carbonization (HTC) technologies for producing value-added carbonaceous material (hydrochar) from coal waste and sewage sludge (SS) waste might be a long-term recycling strategy for hydrogen storage applications, cutting disposal costs and solving waste disposal difficulties. In this study, hydrochars (HC) with high carbon content were produced using a combination of optimal HTC (HTC and Co-HTC) and chemical activation of coal tailings (CT), coal slurry (CS), and a mixture of coal discard and sewage sludge (CB). At 850 °C and 800 °C, respectively, with a KOH/HC ratio of 4:1 and a residence time of 135 min, activated carbons (ACs) with the highest Brunauer–Emmett–Teller specific surface (SBET) of 2299.25 m2g− 1 and 2243.57 m2g− 1 were obtained. The hydrogen adsorption capability of the produced ACs was further studied using gas adsorption isotherms at 77 K. At 35 bars, the values of hydrogen adsorbed onto AC-HCT (AC obtained from HTC of CT), AC-HCS (AC obtained from HTC of CS), and AC-HCB (AC obtained from HTC of the blending of coal discard (CD) and SS) were approximately 6.12%, 6.8%, and 6.57% in weight, respectively. Furthermore, the cost of producing synthetic ACs for hydrogen storage is equivalent to the cost of commercial carbons. Furthermore, the high proportion of carbon retained (>70%) in ACs synthesized by HTC from CD and SS precursors should restrict their potential carbon emissions.