High-quality transparent conductive materials are beneficial to improve the charge transfer and light transmittance and reduce the interface defects as well as the production cost of optoelectronic devices. A high threshold thickness of metal layer in oxide/metal/oxide (OMO) compound thin films leads to strong reflectance, especially in the near-infrared region, limiting the broad-spectrum device applications. Here, we propose a novel Zn doping strategy using the low-cost single-target sputtering technology to achieve the growth of Ag−Zn thin films (i.e., Zn-doped Ag) and introduce a trace amount of O 2 to further obtain ultrathin Ag−Zn(O) films (thin-film thickness d ≤ 5 nm), which greatly improves the broad-spectrum characteristics of OMO films. Heterogeneous metal and gas doping technology effectively promotes the formation of two-dimensional continuous film growth. By combining the ultrathin Ag−Zn(O) layer with the MGZO (i.e., Mg-and Ga co-doped ZnO) oxide film grown by reactive plasma deposition, a typical broad-spectrum MGZO/Ag−Zn(O)/MGZO (50/5/50 nm)-OMO compound thin film exhibits an average transmittance of 91.6% in the wavelength range of 400−1200 nm and low sheet resistance. The broad-spectrum organic solar cells based on MGZO/Ag−Zn(O)/MGZO electrodes present a high power conversion efficiency of 15.35%, superior to those devices based on single-layer oxide electrodes. The distinguished performances are attributed to the ultrathin Ag−Zn(O) films in OMO, paving the way for applications in broad-spectrum optoelectronic and flexible electronic devices.