Combining　transition　metal　phosphides　(TMPs)　with　carbon　nanotubes　(CNTs)　is　a　promising　and　proven　approach　to　enhance　their　performance　in　the　electrochemical　hydrogen　evolution　reaction　(HER),　due　to　the　excellent　conductivity　and　stability　of　CNTs.　Generally,　the　deep　oxidation　of　CNTs　to　form　oxygen-containing　groups　on　their　surface　is　indispensable　before　combining　them　with　TMPs.　However,　such　approaches　inevitably　introduce　a　large　number　of　defects　to　CNTs　and　apparently　decrease　their　stability　and　electrical　conductivity.　Hence,　fabricating　TMP–CNT　composites　which　does　not　come　at　the　expense　of　CNTs＇　high　electrical　conductivity　is　quite　desirable.　In　this　work,　alkylated　CNTs　(named　as　ACNT)　functionalized　via　the　Birch　reaction　are　used　to　prepare　the　pearl　necklace-like　NiCo2P2–ACNT　composites　for　electrocatalysts　toward　HER　in　acidic　and　alkaline　conditions,　respectively.　The　X-ray　photoelectron　spectroscopy,　transmission　electron　microscope,　and　Fourier　transform　infrared　spectroscopy　characterizations　indicate　that　the　ACNTs　are　well　modified　with　functional　groups　and　keep　their　structural　integrity,　thereby　maximizing　their　excellent　conductivity.　Compared　to　bare　NiCo2P2　and　the　NiCo2P2–CNT　composites　prepared　with　mildly　oxidized　CNTs　and　deeply　oxidized　CNTs,　the　NiCo2P2–ACNTs　show　far　better　HER　performance　and　much　faster　kinetics.　©　2018　WILEY-VCH　Verlag　GmbH　&　Co.　KGaA,　Weinheim