A method for applying to an outside surface of a liquid container an anti-leak, self-healing, layered barrier structure intended to inhibit liquid leakage from that container due to an impacting and piercing projectile. The method includes the steps of (a) spray applying to the mentioned container surface a first barrier layer formed of a high-elastomeric material, (b) thereafter, spray applying to the first barrier layer a second, composite-material barrier layer including a body formed of substantially the same high-elastomeric material used in the first barrier layer, and a distribution in that body of a plurality of liquid-imbiber bead elements designed to react with dimensional swelling and related liquid absorption when contacted by any leakage fluid coming from the mentioned container, and (c) thereafter, spray-applying to the second barrier layer a third barrier layer formed of substantially the same high- elastomeric material used in the mentioned first barrier layer, and in the body of the second, composite barrier layer.