Methods for treating erectile dysfunction with therapeutic neuromodulation and associated systems and methods are disclosed herein. Erectile dysfunction can be characterized by the inability to develop and/or maintain an erection during sexual arousal or activity. One aspect of the present technology is directed to methods that at least partially inhibit sympathetic neural activity in nerves innervating the penis of a patient. Sympathetic drive in the patient can thereby be reduced in a manner that treats the patient for erectile dysfunction. Sympathetic nerve activity can be modulated along afferent and/or efferent pathways. The modulation can be achieved, for example, using an intravascularly positioned catheter carrying a therapeutic assembly, e.g., a therapeutic assembly configured to use electrically-induced, thermally-induced, and/or chemically-induced approaches to modulate the nerves.