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The spontaneous organization on a substrate of nanoparticles (NPs) nucleated in a laser-generated plasma results in self-assembling due to both direct specific interactions and to indirect ambient-mediated ones. A number of well-differentiated film morphologies are observed, from isolated NPs to percolated island structures. The distribution of the width of gaps between NPs, or islands formed upon NP coalescence in two representative percolated Au films, is lognormal, indicating that the growth process is random. A finer inspection of similar surface morphologies allows to correlate regularity in gap sizes and surface coverage to differences in film performance as substrates for surface-enhanced Raman spectroscopy.