Abstract: With the increasing demand for energy resources, the development of efficient electrocatalysts has attracted much attention on energy storage and conversion. As a kind of inorganic-organic hybrid materials, recently crystalline metal-organic frameworks (MOF) have been used as electrocatalysts in electrocatalytic reactions due to their abundant metal nodes and organic linkers, high porosity and large surface area. MOF thin films are crucial to achieve effective reactions due to their fast charge transfer and sufficient catalytic sites. Particularly, MOF thin films are coordinated on substrate surfaces by liquid phase epitaxial (LPE) layer by layer (LBL) growth method (called surface-coordinated MOF thin films, SURMOF), which recently have been studied in various fields due to their controlled thickness, preferred growth orientation and homogeneous surface. The backgrounds of electrocatalysis, MOF and SURMOF are briefly introduced at the beginning of this review. Then, the preparation and electrocatalytic applications of SURMOF and their derived thin films (SURMOF-D) are summarized respectively. Owing to the SURMOF based thin films’ tunable structures, controllable thickness and growth orientation, strong coordination interaction between MOF and substrate surface, and compact film, they can provide abundant catalytic sites and fast charge transfer for efficient electrocatalytic activities in oxygen evolution reaction (OER), oxygen reduction reaction (ORR), hydrogen evolution reaction (HER), carbon dioxide reduction reaction (CRR), supercapacitor, tandem electrocatalysis and so on. At the end of the review, SURMOF and SURMOF-D for the electrocatalytic applications are also discussed on the current research challenges and problems to be solved.