Timothy Ray Jones faces multiples charges in his home state of South Carolina of killing his five children and dumping their bodies in another state, the Associated Press news agency reports.
He was arrested on Saturday in Mississippi on unrelated charges.
The children, ages one to eight, were reported missing on Wednesday, when their mother told police she could not get in contact with her ex-husband.
Authorities found the children buried near an Alabama highway after an all-day search on Tuesday, local media reported.
Alabama Department of Public Safety spokesman Sgt Steve Jarrett told a news conference on Tuesday Mr Jones led investigators to the children's bodies.
Smith County, Mississippi, Sheriff Charlie Crumpton told reporters that Mr Jones was stopped at a safety checkpoint on Saturday and was determined to be driving under the influence of drugs,
A deputy found what were believed to be chemicals used to manufacture methamphetamine and a substance believed to be the street drug Spice, Mr Crumpton said.
Investigators also found what appeared to be bleach, hydrochloric acid, blood and possible body fluids inside the vehicle.
When officers ran his vehicle's identification through a national database, police discovered he was wanted in South Carolina "regarding a welfare concern of his children", who were on a national missing persons list.
Mr Jones had told neighbours in South Carolina he was preparing to move out of the state with the children, local media report.
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