The process of radiation‐induced crosslinking of cellulose is found to be highly influenced by radiation dosage and dose as well as by the solvents used and their concentration. The best crease resistance has been obtained in cases when cellulose is crosslinked with acrolein in the vapor phase. Moreover, the process is entirely radiation‐induced and practically no homopolymer is formed. Chemical analysis and investigations of infrared spectra indicate that crosslinking proceeds on vinyl as well as on aldehyde groups of acrolein.