Low-dimensional　semiconductors　provide　promising　ultrathin　channels　for　constructing　more-than-Moore　devices.　However,　the　prominent　contact　barriers　at　the　semiconductor–metal　electrodes　interfaces　greatly　limit　the　performance　of　the　obtained　devices.　Here,　a　chemical　approach　is　developed　for　the　construction　of　p-type　field-effect　transistors　(FETs)　with　low　contact　barriers　by　achieving　the　simultaneous　synthesis　and　integration　of　2D　PdTe2　with　various　low-dimensional　semiconductors.　The　2D　PdTe2　synthesized　through　a　quasi-liquid　process　exhibits　high　electrical　conductivity　(≈4.3　×　106　S　m−1)　and　thermal　conductivity　(≈130　W　m−1　K−1),　superior　to　other　transition　metal　dichalcogenides　(TMDCs)　and　even　higher　than　some　metals.　In　addition,　PdTe2　electrodes　with　desired　geometry　can　be　synthesized　directly　on　2D　MoTe2　and　other　semiconductors　to　form　high-performance　p-type　FETs　without　any　further　treatment.　The　chemically　derived　atomically　ordered　PdTe2–MoTe2　interface　results　in　significantly　reduced　contact　barrier　(65　vs　240　meV)　and　thus　increases　the　performance　of　the　obtained　devices.　This　work　demonstrates　the　great　potential　of　2D　PdTe2　as　contact　materials　and　also　opens　up　a　new　avenue　for　the　future　device　fabrication　through　the　chemical　construction　and　integration　of　2D　components.　©　2021　Wiley-VCH　GmbH