Samuel, 37, was returning home in England after dropping his kids off at school before the tragedy.
"The TTFA and all his former teammates extends deepest condolences to his family in this most hard time". He also had loan spells at Gillingham and Cardiff.
Despite being born in Trinidad and Tobago, Samuel grew up in London, where he joined Charlton Athletic, then moved to Aston Villa in 2007.
Samuel celebrated his 37th birthday in March this year.
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Jlloyd Samuel played for Iranian football team Esteghlal for three years and helped the Blues win title in Iran's Hazfi Cup in 2012 and Iranian league in 2013.
Villa, for whom Samuel played 199 times, primarily at full back, said its players will wear black armbands as a mark of respect in tonight's second leg of their play-off semi-final against Middlesbrough.
"His next of kin have been informed and are now being supported by specially trained officers".
Police said the 54-year-old driver of the van was being treated in hospital for serious injuries.
It read: "We've received some bad news that Jlloyd Samuel died in a auto crash this morning in England".