such technique that is promising for hydrogen production, and comprises an anodic oxygen evolution reaction (OER) and a cathodic hydrogen evolution reaction (HER). [4][5][6][7] This reaction system is generally best aided by noble-metal catalysts such as Pt and RuO 2 /IrO 2 . However, these metals' scarcity and cost severely hinder their widespread application. [8][9][10] Therefore, the development of highly efficient, stable, and inexpensive electrocatalysts to replace precious metals for the integrated HER/OER reaction is crucial to promoting the development of water splitting. [11][12][13] Transitional metal phosphides (TMPs), such as CoP, [14][15][16] Ni 5 P 4 , [17][18][19][20][21][22] and MoP, [23][24][25] have attracted wide attention owing to their low cost, simple preparation, good electrical conductivity, suitable d-electron configuration, moderate intermediate bond energy, and abundant chemical states. [26][27][28] Among them, CoP has demonstrated excellent electrocatalysis because it facilitates the adsorption and desorption of hydrogen and oxygen. However, its weak conductivity and poor corrosion resistance reduce its activity and stability in comparison with Pt-based materials. [29] Carbon-based nanomaterials are widely used in the design of electrocatalysts owing to their excellent resistance to acid and alkali corrosion and good electrical conductivity. [30][31][32] Carbon dots (CDs), as a new type of 0D carbon nanomaterial, have the advantages of simple synthesis and low price. Their graphitized core has good conductivity, and the abundant functional groups on the outer shell can coordinate and cross-link with metal ions to form 3D network structures, which can effectively inhibit the agglomeration and growth of metal nanoparticles. [33] Moreover, doping/modification using heteroatoms (e.g., N, P, F, or Cl) can enhance the electronic interaction between the CDs and the metal, promote electron transfer, and further improve the catalytic performance of the composite material. [34][35][36][37] Note that halogens are used as powerful structural regulators in crystal engineering and other fields owing to their high specificity and directionality. [38][39][40][41] Combining halogens with CDs and introducing them into the design and construction of 3D TMPs composites is expected to control the morphology and surface defects of the composites and increase the number of active sites. [34,39] In addition, traditional powder catalysts often Designing a stable and efficient dual-functional catalyst for the hydrogen evolution and oxygen evolution reactions (HER/OER) is of great significance to the development of hydrogen production by water splitting. This work reports on novel halogen (X = F, Cl, and Br)-doped carbon dots modifying amorphous cobalt phosphide (X-CDs/CoP), which can be tuned by the choice of X-CDs to have urchin, Pinus bungeana, and Albizia julibrissin type structures. The different characteristics of the various X-CDs led to different formation mechanisms and final structures. As a bifunction...