NiFe nanocrystalline films were formed onto Au film via pulsed electrolyte deposition with variable time of relaxation between the sequential pulses. Analysis of anomalous non-liner changes in the NiFe film structure showed the implementation of three mechanisms, resulting in "layer-by-layer", "layer-plus-island", or "island" growth. The change of the interpulse relaxation time provides the possibility to realize all three different mechanisms. The grown NiFe films may have different morphology. The ultrathin NiFe films have nanosized grains and exhibit high uniformity of structure, the films may be also combined of less that 10 nmnanoscale grains and their conglomerates, typically, about 50 nm in size, and, additionally, the film structure, consisting of isolated magnetic islands can be realized. The phenomenological explanation of the differentmechanisms was obtained using atomic-force-microscopy (AFM) approach. It has been demonstrated that the growth mechanism can be controlled by nanocrystallites conglomeration, which is accelerated with increasing the relaxation time. The origin of the conglomeration process is mainly associated with high surface energy of nanosized grains. (c) 2019 The Electrochemical Society.