The physical properties of crosslinked poly(vinyl alcohol)(PVA) by natural dyes as crosslinking agents were investigated and a comparison was made with chemically crosslinked PVA by Polycup 172. It was found that natural anthocyanin and crocin made possible to crosslink PVA physically through the hydrogen bonding of OH in both PVA and natural dyes in the present with NaCl as a catalyst. The water swellability dramatically decreased and the physical crosslinking led to decreasing of crystallinity of PVA. The lowering of thermal stability was noticed in the physically crosslinked PVA compared to chemically crosslinked PVA due to its lower crosslink density. However even natural dyes have polysaccharides in their chain, their thermal stability was higher than uncrosslinked PVA.