water purification has become an urgent task to alleviate this crisis. Solar water evaporation (SWE) is regarded as one of the most promising and clean methods for realizing industrial-grade water purification. [4,5] Several effective SWE material systems have been reported in previous research, including carbon materials, [6][7][8] noble metal nanoparticles, [9][10][11] hydrogel materials, [12][13][14] and semiconducting photothermal materials. [15][16][17][18][19][20] Among them, semiconducting photothermal materials with broad solar absorption, such as the black oxides (e.g., black titanium dioxides [15][16][17][18][19][20] ) and transition metal sulfides, [21][22][23] are particularly attractive for efficiently harvesting and using the solar energy. However, the current techniques of these materials generally exhibit major disadvantages, e.g., photo-degradation, instability, environmental hazards, high cost, or tedious fabrication methods. For example, black TiO 2 materials are generally fabricated using complex and costly reduction methods (e.g., heated at high temperature in pure H 2 or with Mg or Al powders) [24,25] and are vulnerable to chemical instability and photobleaching.Bandgap engineering of semiconductors to achieve abroad solar-spectrum absorption is heavily investigated for wideranging functionalities. Traditional strategies involve high-temperature vapor deposition of multiple compounds of similar lattice structures. [26,27] Other common methods include chemical reduction, doping, or lattice straining. [28,29] However, these methods are limited by the following difficulties: 1) complex and difficult synthetic routes of low production rates and small sample sizes, 2) restricted to specific material systems, 3) small tunable range of bandgap refraining functionalities particularly for achieving wide solar absorption. Therefore, these methods are not applicable for synthesizing massive photothermal materials for SWE. Encouragingly, two recent studies reported that high-entropy design can achieve bandgap reduction by overlapping the electron orbitals of multiple cations: the rare earthbased oxide, (Ce,Gd,La,Nd,Pr,Sm,Y)O 2−δ , displayed a narrowed bandgap (from ≈3 eV of CeO 2 down to ≈2 eV) [30] ; the other transition metal-based oxide, TiZrHfNbTaO 11 , possessed a main bandgap of 2.9 eV (smaller than that of any monoxides). [31] The high-entropy strategy provides a new insight for bandgap engineering. In general, high-entropy materials (HEMs) are defined as solid-solution materials that consist of quasi-equimolar multi component (typically five or more). [32] However, theseThe high-entropy materials have raised much attention in recent years due to their extraordinary performances in mechanical, catalysis, energy storage fields. Herein, a new type of high-entropy hydroxides (e.g., NiFeCoMnAl(OH) x ) that are amorphous and capable of broad solar absorption is reported. A facile one-pot co-precipitation method is employed to synthesize these amorphous high-entropy hydroxides (a-HEHOs) under ambient c...