Big Bang nucleosynthesis in the presence of decaying relic neutral particles is examined in detail. All non-thermal processes important for the determination of light-element abundance yields of 2 H, 3 H, 3 He, 4 He, 6 Li, and 7 Li are coupled to the thermonuclear fusion reactions to obtain comparatively accurate results. Predicted light-element yields are compared to observationally inferred limits on primordial light-element abundances to infer constraints on the abundances and properties of relic decaying particles with decay times in the interval 0.01 sec < ∼ τX < ∼ 10 12 sec. Decaying particles are typically constrained at early times by 4 He or 2 H, at intermediate times by 6 Li, and at large times by the 3 He/ 2 H ratio. Constraints are shown for a large number of hadronic branching ratios and decaying particle masses and may be applied to constrain the evolution of the early Universe.