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Fluorescent probes capable of precise detection of atherosclerosis (AS) at an early stage and fast assessment of anti‐AS drugs in animal level are particularly valuable. Herein, a highly bright aggregation‐induced emission (AIE) nanoprobe is introduced by regulating the substituent of rhodanine for early detection of atherosclerotic plaque and screening of anti‐AS drugs in a precise, sensitive, and rapid manner. With dicyanomethylene‐substituted rhodanine as the electron‐withdrawing unit, the AIE luminogen named TPE‐T‐RCN shows the highest molar extinction coefficient, the largest photoluminescence quantum yield, and the most redshifted absorption/emission spectra simultaneously as compared to the control compounds. The nanoprobes are obtained with an amphiphilic copolymer as the matrix encapsulating TPE‐T‐RCN molecules, which are further surface functionalized with anti‐CD47 antibody for specifically binding to CD47 overexpressed in AS plaques. Such nanoprobes allow efficient recognition of AS plaques at different stages in apolipoprotein E‐deficient (apoE−/−) mice, especially for the recognition of early‐stage AS plaques prior to micro‐computed tomography (CT) and magnetic resonance imaging (MRI). These features impel to apply the nanoprobes in monitoring the therapeutic effects of anti‐AS drugs, providing a powerful tool for anti‐AS drug screening. Their potential use in targeted imaging of human carotid plaque is further demonstrated.

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