Abstract-Threshold and ambiguity phenomena are studied in Part I of this paper where approximations for the mean-squared error (MSE) of the maximum-likelihood estimator are proposed using the method of interval estimation (MIE), and where approximate upper and lower bounds are derived. In this part, we consider time-of-arrival estimation and we employ the MIE to derive closed-form expressions of the begin-ambiguity, end-ambiguity and asymptotic signal-to-noise ratio (SNR) thresholds with respect to some features of the transmitted signal. Both baseband and passband pulses are considered. We prove that the begin-ambiguity threshold depends only on the shape of the envelope of the ACR, whereas the end-ambiguity and asymptotic thresholds only on the shape of the ACR. We exploit the results on the begin-ambiguity and asymptotic thresholds to optimize, with respect to the available SNR, the pulse that achieves the minimum attainable MSE. The results of this paper are valid for various estimation problems.Index Terms-Maximum likelihood estimator, mean-squarederror, nonlinear estimation, optimal signal design, signal-to-noise ratio, threshold and ambiguity phenomena, time-of-arrival.