For the preparation of hardened films which can be applied as a binder for flame-resistant materials such as silica, linseed oil was subjected to a low temperature plasma treatment with argon, or oxygen gas. The film was produced much faster than so-called drying of oil in air. The SEM analysis for silica particles embedded in the hardened film after plasma treatment showed that the silica particles were immobilized on substrate and were evenly dispersed. The FT-IR spectral analysis for the plasma-treated linseed oil films demonstrated that the radicals which were formed during the plasma treatments caused the linseed oil to be cross-linked, and the plasmas attacked carbon chains of the oil randomly without focusing on specific vulnerable bonds such carbon double and carbonyl bonds intensively unless exposure times of the plasmas were prolonged too much, while the cross-linking of the air-dried film was considered to occur at the well-known typical sites, i.e., carbon-carbon double bond and ${alpha}$-methylene carbon. Burning times, as a measure of flame/fire resistance, of silica-filled cellulose substrates, increased with increasing contents of silica.