The favorable self-adhesiveness of resin-modified glass ionomers (RMGIs) might be even further improved if the time-consuming and technically sensitive etch-and-rinse pre-treatment step with polyalkenoic acids could be avoided. We undertook this study to assess the effectiveness of an experimental self-etch adhesive for RMGIs that does not need to be rinsed off. Ultrastructural analysis and micro-tensile bond strength testing to enamel and dentin of a RMGI restorative material and a RMGI adhesive were performed after 4 different surface pre-treatments: no conditioning; 25% polyalkenoic acid; an experimental self-etch adhesive; and 37.5% phosphoric acid followed by the experimental self-etch adhesive. The use of an experimental self-etch adhesive increased the bond strength of RMGIs, especially after an additional conditioning step. Interfacial analysis showed the formation of a thin hydroxyapatite-containing hybrid layer. The self-etch technique enhances the user-friendliness of RMGIs and lowers their technique-sensitivity, while maintaining desirable characteristics of the conventional etch-and-rinse approach with polyalkenoic acids.