We present new visible and near-infrared spectroscopic measurements for 252 near-Earth (NEO) and Mars-crossing (MC) objects observed from 1994 through 2002 as a complement to the Small Main-Belt Asteroid Spectroscopic Survey (SMASS, http://smass.mit.edu/). Combined with previously published SMASS results, we have an internally consistent data set of more than 400 of these objects for investigating trends related to size, orbits, and dynamical history. These data also provide the basis for producing a bias-corrected estimate for the total NEO population (Stuart and Binzel, 2004, Icarus 170, 295–311). We find 25 of the 26 Bus (1999, PhD thesis) taxonomic types are represented, with nearly 90% of the objects falling within the broad S-, Q-, X-, and C-complexes. Rare A- and E-types are more common in the MC than NEO population (about 5% compared to <1%) and may be direct evidence of slow diffusion into MC orbits from the Flora and Hungaria regions, respectively. A possible family of MC objects (C-types) may reside at the edge of the 5:2 jovian resonance. Distinct signatures are revealed for the relative contributions of different taxonomic types to the NEO population through different source regions. E-types show an origin signature from the inner belt, C-types from the mid to outer belt, and P-types from the outer belt. S- and Q-types have effectively identical main-belt source region profiles, as would be expected if they have related origins. A lack of V-types among Mars-crossers suggests entry into NEO space via rapid transport through the ν6 and 3:1 resonances from low eccentricity main-belt orbits, consistent with a Vesta origin. D-types show the strongest signature from Jupiter family comets (JFC), with a strong JFC component also seen among the X-types. A distinct taxonomic difference is found with respect to the jovian Tisserand parameter T, where C-, D-, and X-type (most likely low albedo P-class) objects predominate for T⩽3. These objects, which may be extinct comets, comprise 4% of our observed sample, but their low albedos makes this magnitude limited fraction under-representative of the true value. With our taxonomy statistics providing a strong component to the diameter limited bias correction analysis of Stuart (2003, PhD thesis), we estimate 10–18% of the NEO population above any given diameter may be extinct comets, taking into account asteroids scattered into T<3 orbits and comets scattered into T>3 orbits. In terms of possible space weathering effects, we see a size-dependent transition from ordinary chondrite-like (Q-type) objects to S-type asteroids over the size range of 0.1 to 5 km, where the transition is effectively complete at 5 km. A match between the average surface age of 5 km asteroids and the rate of space weathering could constrain models for both processes. However, space weathering may proceed at a very rapid rate compared with collisional timescales. In this case, the presence or absence of a regolith may be the determining factor for whether or not an object appears “space weathered.” Thus 0.1 to 5 km appears to be a critical size range for understanding the processes, timescales, and conditions under which a regolith conducive to space weathering is generated, retained, and refreshed.