Sorry, no online dictionaries contain the exact phrase opposite of smirk.
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Reverse dictionary results:
1. frown
2. scowl
3. grimace
4. glower
5. beetle-browed
6. lour
7. brinded
8. cringing
9. frowning
10. glowering
11. grimacing
12. grinningly
13. pout
14. scowling
15. sulking
16. wincing
17. frown on
18. frown upon
19. frowner
20. frowny
21. gaping
22. gaum
23. gawm
24. gawp
25. gloat
26. gloating
27. glout
28. gorm
29. gove
30. grin
31. grinning
32. grinny
33. gutturally
34. look
35. murmurously
36. raspy

You can look up the words in the phrase individually using these links:   opposite ?   of ?   smirk ?
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Not helpful? You might try using the wildcards * and ? to find the word you're looking for. For example, use
oppo*to search for words beginning with oppo, or
*mirkto search for words ending with mirk
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