Herein, entire near infrared‐I (NIR‐I) electrochemiluminescence (ECL) enhancement of gold nanoclusters (Au NCs) is achieved by continuously regulating the plasmon resonance absorption wavelength of gold nanorods (Au NRs) to precisely match ECL emission wavelength of Au NCs (abbreviated as Au NCs/Au NRs), which challenges the drawbacks of traditional single wavelength ECL enhancement strategy. Interestingly, within the range of 670 nm to 820 nm, the ECL intensity of Au NCs/Au NRs is 3 ~ 4 times higher than that of individual Au NCs due to the acceleration of electron‐hole recombination and radiation transition rate through high energy electromagnetic field. As a proof of concept, the Au NCs/Au NRs with the ECL emission of 670 nm is employed as high‐efficiency ECL emitter to achieve high‐resolution ECL image and construct biosensor for realizing ultrasensitive detection of matrix metalloproteinase‐2 (MMP‐2) related to liver failure. Significantly, the proposed ECL enhancement strategy effectively enhances the ECL emission of metal nanoclusters (M NCs) over a wide wavelength range and advances a new path for other tunable nanomaterials to enhance the ECL emission of M NCs, which is expected to be applied to in the field of multispectral ECL imaging, multimodal optoelectronic devices and spectrum‐resolved multiplexed biosensing systems.