Prince William said he hoped they would realize "some of us need a helping hand" in a recent interview with the Sunday Times.
Like his mother Princess Diana did when he was 11, the prince has been considering when it might be appropriate to take them to a homeless shelter.
This month, he will begin a new five-year initiative to address the problem.
The interview coincides with the release, for Father's Day, of a new portrait of the Prince beaming with his three children from Kensington Palace.
During his first interview as Prince of Wales, with the Sunday Times, he revealed that he had discussed the homeless with his three children, Prince George, Prince Louis, and Princess Charlotte, on the way to and from school.
"When is the right time to bring George or Charlotte or Louis to a homeless organization?" he pondered as he left the house this morning.
I intend to expose them to it as soon as I am able to fit it into their academic schedule. We discuss our observations on the way to and from school.
We used to speak about the individuals we saw sitting outside of London stores as we drove back and forth between the city.
To the kids, I'd ask, "Why are they there?" Just what is going on? He further, saying, "I think it's in all our interests, it's the right thing to do, to expose the children, at the right stage in the right dialogue, so they have an understanding."
As a result, "they [will] grow up knowing that actually, do you know what, some of us are very fortunate, and some of us need a little bit of a helping hand, and some of us need to do a bit more where we can to help others improve their lives."
As patron of the Passage, an organization that helps the homeless in London, the prince would be continuing a tradition started by his mother, Diana, Princess of Wales, when she accompanied him and his brother there in 1993.
This past year, he reflected on the incident, saying, "My mother introduced me to the problem of homelessness from such an early age, and I'm really glad she did.
I think she'd be upset that we haven't made more progress in preventing and combating homelessness since she was interested in it.
The Royal Foundation, a foundation founded by the prince and his wife, will debut "a really big project" later this month. It is his sincere wish that this will lead to "improved living conditions all across the country for people who need that first rung on the ladder."
This is a shift in focus for the prince, who has been vocal about mental health issues for the past few years.
He plans for part of his effort to focus on reducing youth homelessness, which is of great interest to him. Centerpoint's freedom of information requests to local governments revealed that 122,000 people between the ages of 16 and 24 were either homeless or at risk of becoming homeless.
He stated, "I think 122,000 is a number that is way too high." To prevent this from becoming irreversible, we must take preventative measures now.
When questioned further, the prince said that social housing is "absolutely" on the agenda for the Duchy of Cornwall, the estate provided to the heir to the throne that provides him with an income.
After unveiling a homeless-charity project for young people in the workforce or an apprenticeship who lack access to affordable accommodation, the prince gave an interview to the newspaper.
In the past, Prince William, patron of the homeless organization Centrepoint, made headlines by sleeping rough in Blackfriars, London, for a single night.
He is also sporting the traditional crimson tabard of London Big Issue vendors.