We herein develop a two-in-one molecular design strategy for facile synthesis of 2D imine based covalent organic frameworks (COFs). The integration of two different functional groups (i.e., formyl and amino groups) in one simple pyrene molecule affords a bifunctional building block: 1,6-bis(4-formylphenyl)-3,8-bis(4-aminophenyl)pyrene (BFBAPy). Highly crystalline and porous Py-COFs can be easily prepared by the self-condensation of BFBAPy in various solvents, such as CH2Cl2, CHCl3, tetrahydrofuran, methanol, ethanol, acetonitrile, and dimethylacetamide, etc. The current work, to the best of our knowledge, is a rare case of COF synthesis that exhibits excellent solvent adaptability. Highly crystalline Py-COF thin films have been facilely fabricated on various substrates and exhibit potential applications in hole transporting layers for perovskite solar cells. Furthermore, the versatility of this two-in-one strategy was also verified by two additional examples. The current work dramatically reduces the difficulty of COF synthesis, and such two-in-one strategy is anticipated to be applicable for the synthesis of other COFs constructed by different building blocks and linkages.