Optimal RF flip angles of the NMR CRAZED pulse sequence for multiple spin-echoes (MSEs) and intermolecular multiple quantum coherences (iMQCs) of different orders were investigated theoretically and experimentally. An analytical expression for the dependence of signal intensities on RF pulse flip angles was derived for the cases when higher-order expansion terms of Bessel functions can be neglected from a combination of dipolar demagnetizing field treatment and product operator formalism. Theoretical predictions for both the relative signal intensities and the optimal flip angles at which the signal intensities are maximized are found to be in excellent agreement with experimental results.