Multiferroic　materials　have　great　potential　in　non-volatile　devices　for　low-power　and　ultra-high　density　information　storage,　owing　to　their　unique　characteristic　of　coexisting　ferroelectric　and　ferromagnetic　orders.　The　effective　manipulation　of　their　intrinsic　anisotropy　makes　it　promising　to　control　multiple　degrees　of　the　storage　＂medium＂.　Here,　we　have　discovered　intriguing　in-plane　electrical　and　magnetic　anisotropies　in　van　der　Waals　(vdW)　multiferroic　CuCrP2S6.　The　uniaxial　anisotropies　of　current　rectifications,　magnetic　properties　and　magnon　modes　are　demonstrated　and　manipulated　by　electric　direction/polarity,　temperature　variation　and　magnetic　field.　More　important,　we　have　discovered　the　spin-flop　transition　corresponding　to　specific　resonance　modes,　and　determined　the　anisotropy　parameters　by　consistent　model　fittings　and　theoretical　calculations.　Our　work　provides　in-depth　investigation　and　quantitative　analysis　of　electrical　and　magnetic　anisotropies　with　the　same　easy　axis　in　vdW　multiferroics,　which　will　stimulate　potential　device　applications　of　artificial　bionic　synapses,　multi-terminal　spintronic　chips　and　magnetoelectric　devices.　Manipulating　electrical　and　magnetic　anisotropies　will　stimulate　multi-terminal　device　applications.　Here,　the　authors　discover　axis　dependence　of　current　rectifications,　magnetic　properties　and　magnon　modes　in　van　der　Waals　multiferroic　CuCrP2S6.