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By changing the mixed metal sulfide composi-tion, morphology tuning of an active electrode material can bepossible, which can have a huge impact on its electrochemicalperformance. Here, effective morphology tuning of Ni?Colayered double hydroxide (LDH)/MMoSx(M = Co, Ni, andZn) heteronanostructures is demonstrated by varying thecomposition of MMoSx. Taking advantage of the benefitsassociated with Kirkendall growth and Ostwald ripening,tunable morphologies were successfully achieved. Among theNi?Co LDH/MMoSx(M = Co, Ni, and Zn) heteronanos-tructures, a Ni?Co LDH/NiMoSxcore?shell structuredelectrode delivered a high specific capacity of 404 mAh g?1at 3 mA cm?2and an extraordinary cycling stability (after 10000 cycles) of 93.2% at 50 mA cm?2. In addition, an asymmetric supercapacitor (ASC) device coupled with Ni?Co LDH/NiMoSxas the cathode and Fe2O3/reduced graphene oxide as the anode exhibited excellent cell capacity and extraordinarycycling stability. Moreover, the ASC device provided a very high specific energy of 72.6 Wh kg?1at a specific power of 522.7 Wkg?1and maintained the specific power of 23.5 Wh kg?1at 5357.6 W kg?1, demonstrating its high applicability to energy storagedevices.