Least-squares linear time-invariant (LTI) approximation of discrete-time nonlinear systems is studied in a generalized harmonic analysis setting extending an earlier result based on quasistationary signals. The least-squares optimal LTI model is such that the crosscorrelation between the input and the LTI model output equals the crosscorrelation between the input and the output of the nonlinear system. New results for limits of sample averages of signals are derived via Riemann-Stieltjes integration theory. These results are applied to crosscorrelation and quasistationarity analysis of input-output signals for several important classes of nonlinear systems, including stable finite memory, Wiener and Hammerstein systems. This analysis demonstrates that the assumptions used in the least-squares LTI approximation setup are fairly mild. Finally, an illustrative example is provided. (C) 2004 Elsevier Ltd. All rights reserved.