The behavior of surface and trapped charge that originate during contact electric-field poling of a model guest-host nonlinearly active polymer has been investigated. Charge effects in thin films of pam-nitroaniline doped polymethylmethacrylate were studied during and after the poling process by simultaneous measurement of the current through the poling circuit and the second harmonic generation (SHG) signal from the polymer system. The poling current present in a fresh sample was found to differ in both magnitude and temporal dependence to that observed in the sample during subsequent polings. The magnitude of the steady-state current eventually reached during the poling process was found to depend on temperature and is related to the mobility of charge. A sharp drop-off in SHG signal intensity that occurred when the poling electrodes were grounded is shown to result from the removal of surface charge that orients chromophore dipoles near the surface of the film; the decay in the macroscopic polarization that then occurs is prolonged by charges trapped in the polymer matrix. The build-up of trapped charge explains a memory effect in which the SHG signal relaxation time gradually increased as the film was subjected to multiple polings until a steady-state value was reached. Finally, it is demonstrated that the charges trapped in the polymer matrix are released only after the polymer is heated to high above its temperature of glass transition and the SHG signal has completely decayed away.