Tetteh who rose to prominence in 2009 after guiding Ghana to win the FIFA U-20 World Cup's resignation has come after seven months in charge of the Leone Stars.
The 63-year-old cited personal reasons as to why quitting his position.
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His last game remains a 1-0 loss to Benin in the 2021 Africa Cup of Nations qualifiers in November 2019.
Sellas Tetteh managed only one win in four games he was in charge in the 2022 World Cup qualifiers and the 2021 Africa Cup of Nations qualifications, he lost twice and drew the other.
The 63-year-old had his first spell as coach of Sierra Leone from 2015 to 2017.
The former Liberty Professionals gaffer has also handled the Ghana U17 and U23 national teams and acted as a stop gap coach of the Black Stars in 2008.