The related preparation method for a cross-line array organic molecular device comprises: 1. depositing Si3N4 film on the substrate; 2. spin coating resists on film to photo etch and obtain electrode pattern; 3. with resist for mask, etching the film; 4. evaporating and stripping off metal to obtain cross-line lower electrode; 5. growing sacrificial material; 6. chemical-mechanical polishing last material till the Si3N4 film; 7. spin coating resist to photo etch and obtain upper electrode pattern; 8. similarly, obtaining the upper electrode; 9. releasing the sacrificial material; 10. generating organic molecular material with liquid phase; 11. etching to complete the process.

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