We present the results of generalized spectral fitting (GSF) regressions which estimate normal mode structure coefficients for the observable spheroidal and toroidal free oscillation multiplets below 3 mHz. The size, accuracy, and precision of our new catalogue of modal constraints make it a powerful new tool for assessing and refining three-dimensional Earth models. The estimates include more than 3100 coefficients for 90 multiplets and 25 pairs of coupled multiplets, including several deep mantle overtones previously obscured by fundamental modes. The coefficients constrain mantle structures of both even and odd spherical harmonic degrees, through degree 12 in some cases. Improvements in accuracy and precision have been achieved with three innovations: the development of GSF, an enhancement of the established spectral fitting technique which incorporates both Coriolis and structural coupling between multiplets; the application of GSF to an edited, high signal-to-noise and geographically diverse data set of more than 4500 seismograms from 33 high moment earthquakes; and the assignment of coefficient uncertainties using a Monte Carlo method to simulate the effects of seismic noise, theoretical errors, and coefficient covariances. The results of GSF are assessed by examining the internal consistency of estimated coefficients and through comparisons with recent mantle models. The new catalogue of structure coefficients and uncertainties is available as an electronic supplement to this paper and through the University of Colorado internet site. ¿ 1998 American Geophysical Union