Hybrid electro-electroless deposition (HEED) is the unification of electroplating and electroless deposition in a single electrolyte for the reduction of separate and distinct metals/alloys. The novel combination has the capacity to create unique layered and alloyed deposits by having electroplating and electroless deposition each target a different metal ion within the electrolyte. Electroplating from a Co/Ni-P electrolyte has the capacity to produce Co(Ni-P) layers having over 60% Co atomically. Similarly, electroless Ni-P layers produced from the same electrolyte contain atomically at most 2% Co. Both the electroplating and electroless deposition processes can be tuned to allow greater, or lesser, Co alloying in each layer. The sequential deposition of electroplated Co(Ni-P) and electroless Ni-P within the single electrolyte is used herein to produce a compositionally modulated pentalayer deposit. (C) 2015 The Electrochemical Society. All rights reserved.