PURPOSE: To produce directly a silicon-rubber-like tough organogel comprising polyvinyl alcohol or/and polyolefin oxide and reduced in the formation of cracks and crazes by using an organic solvent.

CONSTITUTION: An organogel is produced by dissolving polyvinyl alcohol or/and polyolefin oxide together with optionally a metal salt in an organic solvent of a relative dielectric constant of 30 or above and subjecting the obtained solution to a freezing and thowing treatment while slowing the temperature change during the freeze treatment or/and the thawing treatment. Alternatively, an organogel is produced by dissolving polyvinyl alcohol or/and polyolefin oxide together with optionally a metal salt in an organic solvent having a relative dielectric constant of 30 or above and containing a nonpolar organic solvent and subjecting the obtained solution to a feezing and thawing treatment. The obtained organogel or gel-like electrolyte has a very low impurity content and an excellent quality.