Continuous, non-invasive monitoring of the arterial pulse is a clinical priority for cardiovascular disease, the leading cause of global mortality. Flexible piezoelectric electronic skins can transduce the 1-10 kPa pressure wave into a self-powered voltage, but the best-performing piezoceramics are lead-based, and their toxicity is incompatible with skin contact and with tightening RoHS/REACH regulation. Among lead-free alternatives, the BaTiO3-based solid solution BZT-BCT reaches d33 ≈ 620 pC/N near its tricritical morphotropic phase boundary, rivalling soft PZT while remaining biocompatible. Exploiting this in a wearable confronts a sensitivity-flexibility paradox and three computational walls: the combinatorial explosion of atomic configurations in a disordered solid solution, the band-gap error of affordable density-functional approximations, which corrupts leakage and insulation estimates, and the 0 K nature of standard calculations against a 310 K operating temperature. We review lead-free piezoelectrics, morphotropic-boundary physics and fabricated flexible devices, then argue that equivariant machine-learning interatomic potentials — coupled to a tiered functional hierarchy and finite-temperature lattice dynamics — can survey the full configurational ensemble at body temperature and close the gap to a clinically viable lead-free pulse sensor.