The energetic performance of hexanitrohexaazaisowurtzitane (CL-20) was modulated with two energetic coordination polymers (ECPs), [Cu(ANQ) 2 (NO 3 ) 2 ] and [Ni(CHZ) 3 ](ClO 4 ) 2 , in this study by a two-step method. First, tannic acid polymerized in situ on the surface of CL-20 crystals. Then, [Cu(ANQ) 2 (NO 3 ) 2 ] and [Ni(CHZ) 3 ](ClO 4 ) 2 were hydrothermally formed on the surface of CL-20/TA, respectively. Explosion performance tests show that the impact sensitivity of the coated structure CL-20/TA/[Cu(ANQ) 2 (NO 3 ) 2 ] is 58% less than that of CL-20 with no energy decrease. On the other hand, CL-20/TA/[Ni(CHZ) 3 ](ClO 4 ) 2 can be initiated by a low laser energy of 107.3 mJ (Nd:YAG, 1064 nm, 6.5 ns pulse width), whereas CL-20 cannot be initiated by even 4000 mJ laser energy. This study shows that it is feasible to modify the performance of CL-20 by introducing energetic CPs with certain properties, like high energy insensitive, laser-sensitive, etc., which could be a prospective method for designing high energy insensitive energetic materials in the future.