Hydrogel sensors have broad application prospects in human motion monitoring and sweat composition detection. However, hydrogel-based sensors are faced with challenges such as low accuracy and poor mechanical properties of analytes detection. Based on mussel-inspired chemistry, we synthesized mesoporous silica@polydopamine-Au (MPS@PDA-Au) nanomaterials and designed a self-healing nanocomposite hydrogel to monitor human movement and ascorbic acid detection in sweat. Mesoporous silica (MPS) possess orderly mesoporous structure. Dopamine (DA) polymerized on the surface of MPS to generate polydopamine (PDA), forming the composite material MPS@PDA-Au. This composite was then embedded into polyvinyl alcohol (PVA) hydrogels through a simple freeze-thaw cycle process. The hydrogels have achieved excellent deformable ability (508.6%), self-healing property (90.5%) and mechanical strength (2.9 MPa). The PVA/MPS@PDA-Au hydrogel sensors had the characteristics of fast response time (123.2 ms), wide strain sensing range (0–500%), excellent fatigue resistance and stability in human detection. The detection range of ascorbic acid (AA) in sweat was wide (8.0 μmol/L-100.0 μmol/L) and the detection limit was low (3.3 μmol/L). Therefore, these hydrogel sensors have outstanding application prospects in human motion monitoring and sweat composition detection.