We investigated the dynamical stability of high-multiplicity Kepler and K2 planetary systems. Our numerical simulations find instabilities in ∼20% of the cases on a wide range of timescales (up to 5×109 orbits) and over an unexpectedly wide range of initial dynamical spacings. To identify the triggers of long-term instability in multi-planet systems, we investigated in detail the five-planet Kepler-102 system. Despite having several near-resonant period ratios, we find that mean motion resonances are unlikely to directly cause instability for plausible planet masses in this system. Instead, we find strong evidence that slow inward transfer of angular momentum deficit (AMD) via secular chaos excites the eccentricity of the innermost planet, Kepler-102 b, eventually leading to planet-planet collisions in ∼80% of Kepler-102 simulations. Kepler-102 b likely has a mass >∼0.1M⊕, hence a bulk density exceeding about half Earth's, in order to avoid dynamical instability. To investigate the role of secular chaos in our wider set of simulations, we characterize each planetary system's AMD evolution with a "spectral fraction" calculated from the power spectrum of short integrations (∼5×106 orbits). We find that small spectral fractions (≲0.01) are strongly associated with dynamical stability on long timescales (5×10^9 orbits) and that the median time to instability decreases with increasing spectral fraction. Our results support the hypothesis that secular chaos is the driver of instabilities in many non-resonant multi-planet systems, and also demonstrate that the spectral analysis method is an efficient numerical tool to diagnose long term (in)stability of multi-planet systems from short simulations.