Morphology‐control synthesis is an effective means to tailor surface structure of noble‐metal nanocrystals, which offers a sensitive knob for tuning their electrocatalytic properties. The functional molecules are often indispensable in the morphology‐control synthesis through preferential adsorption on specific crystal facets, or controlling certain crystal growth directions. In this review, the recent progress in morphology‐control synthesis of noble‐metal nanocrystals assisted by amino‐based functional molecules for electrocatalytic applications are focused on. Although a mass of noble‐metal nanocrystals with different morphologies have been reported, few review studies have been published related to amino‐based molecules assisted control strategy. A full understanding for the key roles of amino‐based molecules in the morphology‐control synthesis is still necessary. As a result, the explicit roles and mechanisms of various types of amino‐based molecules, including amino‐based small molecules and amino‐based polymers, in morphology‐control of noble‐metal nanocrystals are summarized and discussed in detail. Also presented in this progress are unique electrocatalytic properties of various shaped noble‐metal nanocrystals. Particularly, the optimization of electrocatalytic selectivity induced by specific amino‐based functional molecules (e.g., polyallylamine and polyethyleneimine) is highlighted. At the end, some critical prospects, and challenges in terms of amino‐based molecules‐controlled synthesis and electrocatalytic applications are proposed.