We present high-dispersion (R ∼ 16,000) optical (3900-8700 Å) spectra of 390 stars obtained with the Palomar 60 inch telescope. The majority of stars observed are part of theSpitzer Legacy Science Program "The Formation and Evolution of Planetary Systems." Through detailed analysis we determine stellar properties for this sample, including radial and rotational velocities, Li I λ6708 and Hα equivalent widths, the chromospheric activity indexR, and temperature- and gravity-sensitive line ratios. Several spectroscopic binaries are also identified. From our tabulations, we illustrate basic age- and rotation-related correlations among measured indices. One novel result is that Ca II chromospheric emission appears to saturate atv sini values above ∼30 km s^-1, similar to the well-established saturation of X-rays that originate in the spatially separate coronal region.