A composition for the preparation of a transparent, non-elastomeric optical article is provided, the composition including: (1) a polyisocyanate component containing one or more different polyisocyanates; and (2) a component that is reactive with isocyanates, including: (a) optionally at least one polyol having a number average molecular weight greater than 500; (b) (i) at least one polyol and/or polythiol and (ii) at least one compound containing both amine and hydroxyl functional groups, wherein the compound (ii) has a number average molecular weight less than 500; and optionally (3) a urethanation catalyst. Multi-step and one-pot methods of preparing a cured, non-elastomeric polyurethane-containing optical article are also provided.