layer with binary components, where the spontaneous phase separation of the electron donor (D) and electron acceptor (A) provide sufficient D/A interfaces for charge dissociation and continuous network for charge transport. [19,20] In principle, a strong absorbance with a broad absorption band of the photoactive layer is a prerequisite to maximize the harvesting of photons, thereby realizing high photocurrent of the OSC device. [21] In the early period, fullerene derivatives dominated the acceptors, which have low absorption ability, the donor materials contributed mainly to the light harvesting. However, common organic semiconductors intrinsically possess narrow absorption window (the full width at half maximum of the absorption spectrum is about 100-200 nm), which makes it very difficult to realize a broad plateau absorption coverage. [19][20][21][22] Therefore, the device performances were severely restrained to ≈12% for the fullerene-based OSCs. [23][24][25][26] Over the past few years, nonfullerene acceptors (NFAs) have witnessed rapid progress owing to their facile synthesis, easily tunable optoelectronic properties, and strong absorption even reaching the nearinfrared (NIR) region. [3] The largely extended absorption range was realized by pairing low bandgap (LBG) NFAs with the wide bandgap (WBG) polymer donors, thus significantly improving the short current density (J sc ) and PCEs. [5][6][7][8][9][10][11][12][13][14][15] However, its further improvement still remains a formidable challenge due to the almost saturated design toolbox of building blocks for brand new donor/acceptor materials and the insufficient light absorption coverage by binary blends. [27] To make the most of the vast existing pool of semiconductors with various bandgaps and overcome the absorption limitations, tandem devices and ternary blend devices were developed. Tandem OSCs improve the light absorption ability by vertical stacking multiple single-junction cells with complementary absorption. [28] By harvesting both high and low energy photons in the separated subcells, tandem OSCs are able to diminish thermalization loss of photonic energy and overcome the Shockley-Queisser (S-Q) limit. [29] The rapid progress in NFAs has boosted the PCE of tandem OSCs approaching 20%. [14] However, the fabrication of tandem OSCs involves complicated multilayer deposition with serious technical challenges, which may limit their industrialization prospect. Alternatively, the ternary blend organic solar cells (TB-OSCs) strike a good balance between light-harvesting enhancement and device fabrication simplicity by directly Ternary blend organic solar cells (TB-OSCs) incorporating multiple donor and/or acceptor materials into the active layer have emerged as a promising strategy to simultaneously improve the overall device parameters for realizing higher performances than binary devices. Whereas introducing multiple materials also results in a more complicated morphology than their binary blend counterparts. Understanding the morphology is crucially im...