The reuse potential for the large annual production of spent coffee grounds (SCGs) is underexploited in most world regions. Hydrochars from SCGs produced via hydrothermal carbonization (HTC) have been recognized as a promising solid fuel alternative. To increase demand, optimization of the HTC and two post-treatment processes, washing and agglomeration, were studied to improve hydrochar in terms of energetic properties, minimizing unwanted substances, and better handling. HTC experiments at three scales (1–18.75 L) and varying process conditions (temperature T (160–250 °C), reaction time t (1–5 h), and solid content %S_o (6–20%) showed that the higher heating value (HHV) can be improved by up to 46%, and most potential emissions of trace elements from combustion reduced (up to 90%). The HTC outputs (solid yield—SY, HHV, energy yield—EY) were modeled and compared to published genetic programming (GP) models. Both model types predicted the three outputs with low error ( 2000–4000 µm) compared to SCGs (only 4%).