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Bayern midfielder Kroos, 24, is widely expected to join Madrid after the World Cup in a deal worth around 20 million euros, although his agent said no deal had yet been agreed, and other clubs are thought to be interested.
Matthaus told Marca he was disappointed that Kroos was leaving Munich and said: "Congratulations to Real Madrid, because they are getting a phenomenal player.
"I would have liked him to stay in Munich. He is very intelligent, he gives passes, has a very good shot. [Cristiano] Ronaldo and [Gareth] Bale will be able to fill their boots. [Arjen] Robben and [Franck] Ribery have done so over the years."
Matthias, a 1990 World Cup-winner with West Germany, said Joachim Low's side, who face hosts Brazil in the semifinals, had a great chance of winning the tournament given the lack of any one outstanding team.
"We are at a World Cup in which there is no team superior to the others," he explained. "Netherlands played a good first game against Spain, but since then have been worse. Brazil played a good first half against Colombia and then fell back.
"We have not seen exceptional teams. Good games, yes, but not dominating teams."
But Matthaus said he still had reservations about the "Spanish" style of play that Low has introduced to the Germany team in recent years.
"I never believed that my country was going to play pretty passing football, like Spain does -- a technical style, one touch, moving the ball around quickly," he said. "We have played in a very technical style in these years, but we have won nothing."
Germany set off for World Cup semifinal
Germany's World Cup squad are heading to Belo Horizonte for the semifinal against Brazil after leaving their base in Santa Cruz Cabralia on Monday.
Germany unsure of starting XI to face Brazil
ESPN FC's Gustavo Hofman speaks about Germany's Joachim Low not being sure of a starting XI to face Brazil.